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Title: Role of Boron in Enhancing the Catalytic Performance of Supported Platinum Catalysts for the Nonoxidative Dehydrogenation of n -Butane

Abstract

Platinum-based supported catalysts for hydrocarbon conversion are among the most effective for selective dehydrogenation and isomerization processes. However, high process temperatures and the possibility of coke formation require catalyst modifications to mitigate such effects. One of the emerging approaches to prevent platinum catalyst deactivation is the use of boron additives that have been proposed to prevent coking. Despite such a valuable property of boron, the mechanisms for extending the catalyst lifetime and the decrease in coke formation based on this method are still poorly understood. The type and transformations of boron species on silica surface were investigated as a function of boron introduction, platinum addition, catalyst activation, and catalytic reactivity by a combination of X-ray photoelectron spectroscopy, electron microscopy, solid-state nuclear magnetic resonance spectroscopy, and density functional theory calculations to uncover the possible role of boron modification in improving the catalytic performance. Catalytic nonoxidative dehydrogenation of n-butane revealed that incorporation of boron improved the catalytic activity (similar to 3x) and stability of Pt/SiO2. The role of boron in enhancing catalytic performance was attributed to facilitating the migration of alkyl groups from platinum catalytic centers to tetrahedrally coordinated boron sites.

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [2];  [2]; ORCiD logo [2];  [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]
  1. Univ. of Delaware, Newark, DE (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC)
OSTI Identifier:
1604985
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 10; Journal Issue: 2; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; DFT; XPS; boron; platinum; solid state NMR; supported catalysts

Citation Formats

Byron, Carly, Bai, Shi, Celik, Gokhan, Ferrandon, Magali S., Liu, Cong, Ni, Chaoying, Mehdad, Ali, Delferro, Massimiliano, Lobo, Raul F., and Teplyakov, Andrew V.. Role of Boron in Enhancing the Catalytic Performance of Supported Platinum Catalysts for the Nonoxidative Dehydrogenation of n -Butane. United States: N. p., 2019. Web. https://doi.org/10.1021/acscatal.9b04689.
Byron, Carly, Bai, Shi, Celik, Gokhan, Ferrandon, Magali S., Liu, Cong, Ni, Chaoying, Mehdad, Ali, Delferro, Massimiliano, Lobo, Raul F., & Teplyakov, Andrew V.. Role of Boron in Enhancing the Catalytic Performance of Supported Platinum Catalysts for the Nonoxidative Dehydrogenation of n -Butane. United States. https://doi.org/10.1021/acscatal.9b04689
Byron, Carly, Bai, Shi, Celik, Gokhan, Ferrandon, Magali S., Liu, Cong, Ni, Chaoying, Mehdad, Ali, Delferro, Massimiliano, Lobo, Raul F., and Teplyakov, Andrew V.. Wed . "Role of Boron in Enhancing the Catalytic Performance of Supported Platinum Catalysts for the Nonoxidative Dehydrogenation of n -Butane". United States. https://doi.org/10.1021/acscatal.9b04689. https://www.osti.gov/servlets/purl/1604985.
@article{osti_1604985,
title = {Role of Boron in Enhancing the Catalytic Performance of Supported Platinum Catalysts for the Nonoxidative Dehydrogenation of n -Butane},
author = {Byron, Carly and Bai, Shi and Celik, Gokhan and Ferrandon, Magali S. and Liu, Cong and Ni, Chaoying and Mehdad, Ali and Delferro, Massimiliano and Lobo, Raul F. and Teplyakov, Andrew V.},
abstractNote = {Platinum-based supported catalysts for hydrocarbon conversion are among the most effective for selective dehydrogenation and isomerization processes. However, high process temperatures and the possibility of coke formation require catalyst modifications to mitigate such effects. One of the emerging approaches to prevent platinum catalyst deactivation is the use of boron additives that have been proposed to prevent coking. Despite such a valuable property of boron, the mechanisms for extending the catalyst lifetime and the decrease in coke formation based on this method are still poorly understood. The type and transformations of boron species on silica surface were investigated as a function of boron introduction, platinum addition, catalyst activation, and catalytic reactivity by a combination of X-ray photoelectron spectroscopy, electron microscopy, solid-state nuclear magnetic resonance spectroscopy, and density functional theory calculations to uncover the possible role of boron modification in improving the catalytic performance. Catalytic nonoxidative dehydrogenation of n-butane revealed that incorporation of boron improved the catalytic activity (similar to 3x) and stability of Pt/SiO2. The role of boron in enhancing catalytic performance was attributed to facilitating the migration of alkyl groups from platinum catalytic centers to tetrahedrally coordinated boron sites.},
doi = {10.1021/acscatal.9b04689},
journal = {ACS Catalysis},
number = 2,
volume = 10,
place = {United States},
year = {2019},
month = {12}
}

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